The neighborhood's borders are defined by the Norfolk Southern tracks on the north, Grant Street on the east, 25th Avenue on the south, and Clark Road on the west.

Distinctive subdivisions within Tolleston include Tarrytown, running for ten blocks north-to-south between Clark Road and Whitcomb Street, and Small Farms at the neighborhood's southern end.

Prior to the founding of Gary in 1906, it was the principal settlement in the region, and Tolleston's Gibson Hotel was used as a base by the officials of US Steel planning the new city.

Custom designed by renowned Modernist architect Edward D. Dart in 1958, the historically Black Episcopal church garnered two architecture awards.

Tolleston is also the home of St. John's (Evangelical) Lutheran Church, located on the corner of 10th Avenue and Taft St.