The park's only season as the home field for an all-professional team occurred in 1872 when the Brooklyn Atlantics joined the National Association of Professional Base Ball Players.

Fred Goldsmith successfully demonstrated his curve ball at the grounds in 1870, a pitch previously thought to have been only an optical illusion.

In an 1865 game, Ned Cuthbert is credited with inventing the slide when he tried avoiding a tag when attempting to steal a base against the Athletic of Philadelphia.

In addition to baseball, the grounds hosted various events and exhibitions; most notably in 1873, when Washington H. Donaldson and two reporters attempted to fly a gas balloon across the Atlantic Ocean.

[5] The Capitoline Grounds opened for baseball in 1864, consisting of two sets of bleachers that were backed by Nostrand Avenue and Halsey Street, and had an approximate capacity of 5,000 people.

[6] In right field stood a circular brick outhouse, and if any player hit a ball over the structure, they were presented with a bottle of Champagne.

On May 5, 1864, the first baseball game at Capitoline was a match between the Atlantics and a field of nine players from other Brooklyn teams chosen by sportswriter Henry Chadwick.

[15] With approximately 20,000 people in attendance, Harry Wright and the Cincinnati Red Stockings attempted to extend their 84-game winning streak against the Atlantics in Brooklyn.

[16] In the top of the 11th inning‚ the Red Stockings scored two runs, giving themselves a 7–5 lead, but the Atlantics countered with three of their own in the bottom half of the 11th, winning the game.

[16] Henry Chadwick wrote an account that on August 16, 1870, Fred Goldsmith demonstrated a new pitch, the curve ball, at the Capitoline Grounds.

"[17] By the 1930s, the established baseball community had given the discovery credit to Candy Cummings, and due to Chapman's age, determined that his demonstration has most likely occurred a few years later.

Barnum as a circus performer, along with fellow balloonist John Wise, collaborated on an attempt to cross the Atlantic Ocean in a hot-air balloon.

Sponsored by the Daily Graphic, the launch was to take place from the Capitoline Grounds, with Wise planning to use a balloon 49 meters (160 feet) tall with a two-compartment enclosed car, but decided to end his involvement with the project.

[19] Donaldson's Atlantic attempt, launched from the Capitoline Grounds accompanied by reporters Alfred Ford and George Lunt, ended up being forced down by a rainstorm, to land on a Connecticut farm.