Canterbury Başpiskoposu olduğunda neredeyse 60 yaşında olan Laud, artık kendi bildiği yolun dışında bir uzlaşmaya yanaşmayacak şekilde ilerlemeye başlar.
Laud was almost 60 years old when he became Archbishop, and having waited to replace George Abbot, was no longer prepared to compromise on any aspect of his policy. Abbot's chaplains had licensed Histriomastix for publication, in 1630; the book had caused scandal when it appeared in late 1632, and one of Laud's early moves was to bring in his own men as censors: Samuel Baker (who was chaplain to William Juxon), William Bray and Matthew Weeks. The operations of the censors, including William Haywood who joined them, were a focus of the Long Parliament as soon as it was convened, and Laud had to answer for Haywood at his own trial.
Whereas Wentworth saw the political dangers of Puritanism, Laud saw the threat to the episcopacy. But the Puritans themselves felt threatened: the Counter-Reformation was succeeding abroad and the Thirty Years' War was not progressing to the advantage of the Protestants. In this climate, Laud's high church policy was seen as a sinister development. A year after Laud's appointment as Archbishop of Canterbury, the ship Griffin left for America, carrying religious dissidents such as Anne Hutchinson, the Reverend John Lothropp and the Reverend Zechariah Symmes.
Laud's policy was influenced by his desire to impose uniformity on the Church of England, which was driven by a belief that this was the duty of his office but, to those of differing views, it came as persecution. Perhaps this had the unintended consequence of garnering support for the most implacable opponents of the Anglican compromise. In 1637, William Prynne, John Bastwick and Henry Burton were convicted of seditious libel and had their ears cropped and their cheeks branded. Prynne reinterpreted the "SL" ("Seditious Libeller") branded on his forehead as "Stigmata Laudis". Laud moved to silence his principal episcopal critic John Williams who was convicted of various offences in Star Chamber; but contrary to Laud's expectation, Williams refused to resign as Bishop of Lincoln, and waited patiently until 1641 when he moved to bring about Laud's downfall.
Charles I towards the end of his life admitted that he had put too much trust in Laud, and allowed his "peevish humours ", and obsession with points of ritual, to inflame divisions within the Church: he warned his son not to rely entirely on anyone else's judgement in such matters. Laud, on his side, could not forgive the King for allowing the execution of Strafford (as Wentworth became), and dismissed him as "a mild and gracious Prince, that knows not how to be or be made great".