Hearing of the great encouragement extended to the arts by Charles I., he determined to visit England in 1629. While there, he lodged with his friend and countryman, George Geldorp the painter, and expected to be presented to the king; but his hopes not being realized, he visited Paris; and meeting no better success there, be returned to his own country, with the intention of remaining there during the rest of his life. Charles, however, having seen a portrait by Vandyck, of the musician, Fic. Laniere, director of the music of the king's chapel, requested Sir Kenelm Digby to invite him to return to England. Accordingly, in 1631, he arrived a second time at London, and was received by the king in a flattering manner. He was lodged at Blackfriars, among the King's artists, where his majesty frequently went to sit for his portrait, as well as to enjoy the society of the painter. The honor of knighthood was conferred upon him in 1632, and the following year he was appointed painter to the king, with an annuity of £200.

Prosperity now flowed in upon the Fleming in abundance, and although he operated with the greatest industry and facility, painting single portraits in one day, he could hardly fulfill all his commissions. Naturally fond of display, he kept a splendid establishment, and his sumptuous table was frequented by persons of the highest distinction. He often detained his sitters to dinner, where he had an opportunity to observe more of their peculiar characteristics, and retouched their pictures in the afternoon. Notwithstanding his distinguished success, he does not appear to have been satisfied with eminence in portrait painting; and not long after his marriage with Maria Ruthven, granddaughter of Lord Gowrie, he went to Antwerp with his lady, on a visit to his family and friends, and thence proceeded to Paris. The fame which Rubens had acquired by his celebrated performances at the Luxembourg, rendered Vandyck desirous to execute the decorations at the Louvre; but on arriving at the French capital, he found the commission disposed of to Nicholas Poussin. He soon returned to England, and being still desirous of executing some great work, proposed to the king through Sir Kenelm Digby, to decorate the walls of the Banqueting House (of which the ceiling was already adorned by Rubens), with the History and Progress of the Order of the Garter. The sum demanded was £8000, and while the king was treating with him for a less amount, the project was terminated by the death of Vandyck, December 9th, 1641, aged 42 years. He was buried with extraordinary honors in St. Paul's cathedral. His high living had brought on the gout during his latter years, and luxury had considerably reduced his fortune, which he endeavored to repair by the study of alchemy. He left property amounting to about £20,000. In his private character, Vandyck was universally esteemed for the urbanity of his manners, and his generous patronage to all who excelled in any science or art, many of whose portraits he painted gratuitously.