The Al Nassr forward won his 197th cap in Friday's (AEDT) opening Euro 2024 qualifier against Liechtenstein, moving him one clear of Kuwait forward Bader Al-Mutawa.
Malaysia's Soh Chin Ann (195 caps) is third on the list, with Ahmed Hassan (184) and Ahmed Mubarak (183) of Egypt and Oman respectively completing the top five.
Ronaldo had equalled Al-Mutawa's record when featuring for Portugal in its FIFA World Cup quarter-final defeat to Morocco in December.
Speaking ahead of the meeting with Liechtenstein at Estadio Jose Alvalade, Ronaldo revealed he contemplated retiring from international football after that defeat.
But he was named in new head coach Roberto Martinez's first squad and made more history when appearing against minnows Liechtenstein in Lisbon.
Ronaldo, who also holds the record for most men's international goals (118), earned his first cap in 2003 when replacing Luis Figo in a friendly against Kazakhstan.
The five-time Ballon d'Or winner, who won Euro 2016 with Portugal, has played against Luxembourg (10 games) more times than any other nation, followed by Spain (nine).
Luxembourg are also the country Ronaldo has scored against the most, finding the net nine times, while he has scored seven times against Lithuania and Sweden.
He has played 47 times for Portugal at major tournaments – 25 times at the European Championships and 22 at the World Cup – and is hopeful of featuring at Euro 2024.
"My biggest wish is to be able to take Portugal as high as possible," Ronaldo said on Wednesday. "I will always play my part when needed.
"Earning records is always a positive thing and it motivated me. I like to break records and will now break another special one. It makes me very proud.
"But beyond [Thursday] I still have plenty of games left. Let's see if the coach still wants to count on me to be available."