We present the results of near-infrared (NIR) imaging and spectroscopic observations of the Galactic supernova remnant Cassiopeia A (Cas A). Applying the method of Principal Component Analysis to our broadband NIR spectra, we identify a total of 61 NIR emission knots of Cas A and classify them into three groups of distinct spectral characteristics: Helium-rich, Sulfur-rich, and Iron-rich groups. The first and second groups are of the circumstellar and supernova ejecta origin, respectively. The third group, which has enhanced iron emission, is of particular interests since it shows intermediate characteristics between the former two groups. We suggest that the Iron-rich group is knots of swept-up circumstellar medium around the contact discontinuity in Cas A and/or supernova ejecta from deep layers of its progenitor star which have recently encountered a reverse shock in the remnant.