A new series of La(1-x)Ce(x)CrO(3) (0.0 <or= x <or=1.0) compounds in nanocrystalline form were synthesized using a two-step synthesis route, involving an initial combustion reaction followed by vacuum heating in the presence of a Zr sponge, which acted as an oxygen getter. For the first time, a homogeneous solid solution formation throughout the entire range was obtained in this series. These compounds were characterized using X-ray diffraction, diffuse reflectance UV visible spectrophotometry, and superconducting quantum interference device magnetometry. The crystallite size for the phase-pure products was confirmed to be approximately 42-44 nm by high-resolution transmission electron microscopy. All compounds (nanocrystalline) in this series are found to be predominantly antiferromagnetic in nature with a remarkable linear increasing trend in Neel temperature from 257 to 281.5 K as a function of decreasing Ce(3+) content. Interestingly, the band gap also shows a linear decrease from 3.21 to 3.02 eV as a function of increasing Ce(3+) concentration in the La(1-x)Ce(x)CrO(3) series.