The expansion, made possible when Austria and other members dropped their objections to the former communist countries joining, officially took place at midnight (22:00 GMT) on Wednesday.
Identification checks at the land borders between Bulgaria and Romania and their neighbouring European Union member countries officially ceased at midnight, providing travellers free access to the rest of the 27-member bloc.
The two Balkan countries partially joined the Schengen Area in March, but open travel was restricted to those arriving only by air or sea.
Romanian and Bulgarian border police at the Giurgiu-Ruse border marked the moment with ceremonies, a sign of the culmination of a 13-year wait for full Schengen membership.
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