The Argentine, 54, overtook the late club legend Luis Aragones on 612, and, accompanied by his own children, was handed a commemorative shirt to mark the new milestone by Aragones’s son before kick-off.
“Legend Simeone,” read the back of the shirt and electronic displays around the stadium as Atletico fans chanted their coach’s name in appreciation for his service.
Simeone, who played for the club in midfield across two spells, took over as coach in 2011.
Known for his competitive – and sometimes abrasive – style, Simeone helped Atletico win La Liga in 2014 and 2021, and the Copa del Rey in 2013.
The coach established Atletico as a team capable of battling with giants Real Madrid and Barcelona for domestic honours.
Before the Simeone era, the last time they won La Liga and the Copa del Rey was in 1996, when they did the domestic double under Radomir Antic.
Simeone also steered Atletico to the 2014 and 2016 Champions League finals, but his side suffered defeat in both against bitter rivals Real Madrid.
He guided the club to Europa League triumphs in 2012 and 2018, as well as two European Super Cups.
This season Atletico have underwhelmed, failing to compete in the title race and suffering a group stage Champions League exit, with speculation Simeone’s reign could come to an end in the summer.