In the summer of 1808 Buckland made his first geological tour. Alone and on horseback he travelled from Oxford across the chalk hills of Berks and Wilts and Dorset to Corfe Castle in the Isle of Purbeck. In the vertical strata of hard white limestone on which that castle stands he recognised the chalk, but the relations of the strata above and below that formation were then unknown. In the following year he explored in the same way a large part of South Devon, visiting the granite of Dartmoor, examining minutely the formations, and collecting specimens of the geology of the district. In 1810 he made a tour through the centre and north of England, examining the then unknown extent of the various strata, and colouring the results on Carey's large map of England.

Other journeys followed in annual succession. Thus in 1813 Buckland, adopting the true Wykehamical fashion of going two and two, made a tour with his friend Mr. W. Conybeare in Ireland. In collaboration with his travelling companion, he published his first important paper—“On the Coasts of the North of Ireland.” Among the organic remains in many of the chalk pits from Moira to Belfast and Larne he discovered some curious siliceous bodies known by the name of “Paramoudra.”