The fabrication of high-performance spherical gradient refractive index (S-GRIN) optics requires nondestructive metrology techniques to inspect the samples. We have developed an angular-scan, swept-source-based, Fourier-domain optical coherence tomography (OCT) system centered at 1318 nm with 5 mm imaging depth capable of 180° polar scan and 360° azimuthal scan to investigate polymeric S-GRIN preforms. We demonstrate a method that enables simultaneous mapping of the group optical thickness, physical thickness, the radially-averaged group refractive index, and the transmitted wavefront of the S-GRIN preforms. The angular scan OCT imaging and metrology enables direct visualization, molding uniformity characterization, and optical property evaluations of the preforms. The results on two generations of S-GRIN preforms are discussed that showcase the evolution of the manufacturing process in response to the OCT metrology feedback.