Ronaldo, who turned 38 last month, won his 197th cap, surpassing Kuwait's Bader Al-Mutawa, as he captained his country to a 4-0 win over Liechtenstein in the Group J qualifier in Lisbon.
The former Real Madrid and Manchester United striker marked the occasion by converting a penalty and adding another second-half goal to move onto 120 goals in internationals.
Ronaldo had been benched by former coach Fernando Santos for the team's final two games at last year's World Cup in Qatar where Portugal lost in the quarter-finals to Morocco.
Thursday marked the first game in charge for new coach Roberto Martinez, who had expressed his faith in Ronaldo's ability to continue delivering for his country.
"I look for commitment," Martinez said this week. "And Ronaldo has huge commitment to the national team, is a major figure for it, and has experience he can pass on."
Ronaldo, who made his Portugal debut in 2003, also holds the world record for the most goals in men's international football with 118.
"I like to break records, I have broken lot of records," he said.
Ronaldo has scored against 46 different international opponents, but never against Liechtenstein.
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