After edging the first session 5-4, 'The Rocket' stormed through the remaining frames with three stunning century breaks to sweep aside Carter without reply.
Elsewhere, Judd Trump made light work of China's Zhou Yuelong with a commanding 10-4 victory after building a strong 6-3 lead in the opening session.
One of the day's biggest surprises came from Pang Junxu, who recovered from 5-3 down to beat compatriot Zhang Anda 10-7 in a composed display.
Shaun Murphy also secured a spot in the next round with a dominant 10-4 win over Welsh qualifier Daniel Wells that showed signs of a deep Crucible run.
In matches that'll conclude tomorrow, Belgian star Luca Brecel and Ryan Day are locked in a tight battle with the Welshman holding a narrow 5-4 lead. Meanwhile, Woollaston trails local rival Selby 5-4.
Results
Judd Trump 10-4 Zhou Yuelong
Ronnie O'Sullivan 10-4 Ali Carter
Shaun Murphy 10-4 Daniel Wells
Zhang Anda 7-10 Pang Junxu
Mark Selby 5-4 Ben Woollaston*
Luca Brecel 4-5 Ryan Day*
*After first session.