The 23-year-old won the omnium at the UCI Track Cycling World Championships in Denmark on Saturday to back up her win in the elimination the day prior.
She joins Alison Shanks and Aaron Gate as New Zealanders with double rainbow jersey wins on the track.
The men's sprint trio of Ethan Mitchell, Sam Webster and Eddie Dawkins stand alone with three world championship titles, although Wollaston has the chance to join them with one event remaining on Monday (NZ time).
In the four-discipline omnium, Wollaston was ninth in the 7.5km scratch race, before topping the tempo race, winning 10 of the 26 sprints and gaining a lap on the field.
Wollaston stayed calm as the attacks came in the pivotal 20km points race, with points awarded for sprints every 10 laps and 20 bonus points for lapping the field.
Great Britain's Jessica Roberts went solo to gain a lap and an eight-point lead but Wollaston stayed with her plan, scoring points on six of the eight sprints including winning the double-points final sprint.
Wollaston finished on 131 points, 11 clear of Roberts with Norway's Anita Stenberg third.
"As I was yesterday, I am blown away and still a little bit lost for words," Wollaston said.
"I knew after yesterday that the form was there but to put it together on omnium day is a different story.
"I am just really happy with today's performance . When Jess [Roberts] went for the lap, I was questioning whether I had it in the final. But I had to try to stay calm and back my last sprint.
"I started the day with not such a great scratch race but managed to back it up with a few good races after that."
Wollaston returns on the final day of competition to contest the individual points race.