In an effort to raise funds on behalf of the Virginia Company, Rebecca Rolfe, as Pocahontas was now known, sailed to England in the spring of 1616 with her husband John Rolfe; Deputy Governor Dale; a retinue of young Indian women, some of whom would remain in England; and the priest Uttamatomakkin , a brother-in-law of Powhatan sent by the paramount chief as an observer. In particular, Uttamatomakkin was tasked with finding John Smith, meeting the English king, viewing the English god, and conducting a census of both the Englishmen and their trees. (An earlier Indian visitor, who saw only London and the Thames River, had mistakenly reported that there were next to no trees in England, explaining why the English sought timber in Virginia.) Uttamatomakkin would accomplish the first two objectives but fail with the rest, and his encounters with evangelistic clergymen such as Reverend Samuel Purchas would turn his sympathies forever against the English.

After landing in Plymouth in September 1616, the party traveled overland to London, so Pocahontas saw a good deal of southern England. Once in London, she was lodged and clothed at the Virginia Company's expense and an engraving was made of her by Simon van de Passe that was intended for circulation by the company in its fund-raising efforts. Pocahontas also was introduced into English society, presumably by the lieutenant governor and his wife, Lady Elizabeth Dale, a distant cousin of the late Queen Elizabeth. The wife of Virginia's governor, Thomas West, baron De La Warr, may also have helped sponsor Pocahontas. While John Smith later claimed that he could have presented the young woman to the English aristocracy, he never had anything like the social clout of either the Dales or the De La Warrs.

Pocahontas caused a sensation among an English upper crust that was always in search of novelty and amusement. She had an audience with the bishop of London, John King, who, in the words of Purchas, entertained her "beyond what I have seen in his great hospitality afforded to other Ladies." She and Uttamatomakkin also met King James I at Whitehall Palace and impressed him sufficiently that they were invited to attend, on January 6, 1617, his Twelfth Night masque, a formal costume ball held every year on the last night of the Christmas season. "Well placed" by the king—in other words, seated among important people—they viewed The Vision of Delight by Ben Jonson, which was performed at the ball. Although a century later Robert Beverley Jr. wrote that King James was angry with John Rolfe for presuming to marry a "princess," there is no contemporary evidence to suggest that the king was angered by the marriage and that Pocahontas was regarded as anything like royalty. One Englishman who met her referred to her only as "the Virginian woman," refusing to acknowledge her as a lady.

Even John Smith took little trouble to pay his respects to his former friend. Living in London himself, he waited several months before calling on her; in his 1624 account, he claimed that he had been too busy. When he finally made his appearance, Pocahontas was so angry with him that she retired to another room to regain her composure. Their conversation, once it began, soon degenerated into her flinging taunts at him about his shabby treatment of her father. Smith ended his account of the visit with her telling him that "your countrymen will lie much [often]."

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If Smith was an accurate reporter—he wrote about the conversation seven years after it happened—then Pocahontas may have been experiencing some disillusionment with her husband's people. By the time Smith came around, she and her family had moved to Brentford, then a small village outside London. Later writers have claimed that her health was failing in the capital's smoky environs, although this is unlikely given the fact that Pocahontas had grown up in smoky Indian houses. It is more probable that her novelty among the upper classes had faded, and, absent rich sponsors, the Virginia Company was forced to transfer her to cheaper accommodations. Indirect evidence also suggests that she was in good health at that time. Though they were already planning to return to Virginia, a week before they departed the Rolfes were awarded a large grant by the Virginia Company to start a mission. As part of such an enterprise, Pocahontas would have been expected to serve the dual roles of interpreter and housemother, which would have been a strenuous assignment for someone who was ill or dying.

After a two-month delay because of bad weather, the Rolfes and Uttamatomakkin embarked for Virginia in March 1617. Pocahontas was rumored to have regrets about leaving London, but that may have been wishful thinking on the part of some Englishmen. In the end, though, she took ill. Pocahontas, then about twenty-one years old, was taken ashore at Gravesend, down the Thames River from London, where she died. On March 21, she was interred under the chancel of St. George's Church in Gravesend, a burial place indicating that she was considered a lady. Her son, Thomas, too sick himself to travel, remained in England. (He finally sailed for Virginia in 1635, but it was thirteen years after his father's death.) Uttamatomakkin, meanwhile, returned to Virginia with John Rolfe and Samuel Argall and reported to Powhatan's brother, Opechancanough, in such negative terms about his experience that the English attempted to discredit him. The ships that carried Argall, Rolfe, and Uttamatomakkin back to Virginia also brought to the colony an epidemic of hemorrhagic dysentery which colonists called bloody flux and which Argall referred to as "a great mortality"; this epidemic may have been the cause of Pocahontas's death.