The Cardinals went 83–79 during the season and finished sixth in the National League, 12 games behind the Los Angeles Dodgers.

On July 12, the Cardinals hosted the 1966 Major League Baseball All-Star Game at their new stadium, in 105 degree heat and humidity, with the NL defeating the AL, 2–1 in ten innings.

Later derided as a facsimile of the bland, cookie-cutter "multi-purpose stadia" built in multiple locations of the United States during the 1960s and 1970s, Busch Memorial achieved a measure of popularity among St. Louis fans in a way that its cousins in Philadelphia, Atlanta, Pittsburgh, and Cincinnati did not, perhaps due in part to the success of the teams which played there, and perhaps also due to the distinctive roof arches added by architect Edward Durrell Stone — unique touches meant to echo the city's new iconic monument (completed at nearly the same time), the Gateway Arch.

Pitcher Bob Gibson and outfielder Curt Flood won Gold Gloves this year.

Infielders Other batters Coaches Note: Pos = Position; G = Games played; AB = At bats; H = Hits; Avg.