The Argentine coach enjoyed his 308th victory in charge of the club in Atletico's 2-0 LaLiga triumph.
An own goal from Alfonso Pedraza and a fine strike from Joao Felix secured the win, sending Atletico five points clear at the top of the table.
In so doing, Simeone matched the esteemed Luis Aragones as the Atletico head coach with the highest number of victories in all competitions.
Simeone's latest win came in his 512th match in charge. Aragones, the only man to take charge of more games, reached 308 wins in 612 matches at a rate of 50.3 per cent.
Atletico have drawn 120 times and lost only 84 games under Simeone, who took over on December 23 in 2011 and has since become the club's most successful coach.
Aragones, a star for Atletico as a player, also won six trophies as head coach. Simeone, with seven, is the only man with more.
In a little over nine years in charge, the former Argentina midfielder has led Atletico to two UEFA Super Cups, two Europa Leagues, one Supercopa de Espana, one Copa del Rey and, most famously, their only LaLiga title in the past 25 years back in 2013-14.
Simeone has helped to tip the balance of power somewhat in Spain's capital. He is the only coach to have won three finals against Real Madrid in three different competitions: the Copa del Rey (2013), the Supercopa de Espana (2014) and the UEFA Super Cup (2018).
He has twice faced them in the Champions League final, too, losing after extra time in 2014 and on penalties two years later.
Among South American coaches, only Helenio Herrera (359) has taken charge of more LaLiga matches than Simeone (351).
All of those have been with Atletico, of course. There are just two coaches to oversee more LaLiga games at a single club: Aragones at Atletico (407) and Miguel Munoz at Real Madrid (424).
Munoz won 357 of his 605 games in charge of Los Blancos in all competitions, so Simeone has a little way to go to surpass that tally. Still, he has already won more games than Barcelona record-holder Johan Cruyff, who won 244 times out of 421 matches.
Antoine Griezmann is the player to score the most goals under Simeone at Atletico, with 133 in all competitions.
The rest of the top five includes Diego Costa (75), Radamel Falcao (58), Koke (44) and Saul Niguez (43).
Koke leads the way for assists, with 95, comfortably clear of Griezmann (46), Gabi (44), Angel Correa (43) and Juanfran (32).