Around 1665, Verrio moved to the region of Toulouse where he was commissioned to decorate the Château de Bonrepos, the property of Pierre-Paul Riquet, promoter of the Canal du Midi.

Thanks to Montagu, Verrio made his English debut working for aristocrats such as the 1st Earl of Arlington (Euston Hall and Arlington House, now destroyed) and the 1st Duke of Lauderdale (Ham House, now a property of The National Trust), and rapidly acquired the royal patronage of Charles II.

Soon afterwards he was engaged to decorate the North Range of Windsor Castle, where he collaborated with the architect Hugh May and the sculptor Grinling Gibbons.

This was the most important commission of his entire career: twenty ceilings, three staircases, the King's Chapel and St George's Hall for which he was paid the colossal sum of £10195 8s 4d.

On the succession of James II, Verrio continued his royal service and decorated Whitehall Palace (burnt in 1698) and Henry VIII's Chapel at Windsor (destroyed).

In France, his work can be seen in Toulouse at the musée des Augustins and at Saint Exupère's church and in Paris, where he painted some of the vaults of the Hôtel Brûlart.