This data release contains geochemical data, thin section images, and 40Ar/39Ar isotopic data from bedrock samples in the Orange-Milford Belt of south-central Connecticut. The geochemical data comprise whole-rock major oxide and trace element abundances in 111 samples. Pairs of images in plane-polarized light and cross-polarized light are included for 90 thin sections. Step-heated 40Ar/39Ar analyses of mineral separates/concentrates from 10 different hand samples are also included and comprise 8 analyses of muscovite/sericite, 3 analyses of potassium feldspar, and 2 analyses of actinolite.