A new series of La1-xCexCrO3 (0.0 <= x <= 10) 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 similar to 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 Ce3+ content. Interestingly, the band gap also shows a linear decrease from 3.21 to 3.02 eV as a function of increasing Ce3+ concentration in the La1-xCexCrO3 series.