The plane of trans-Stilbene (TSB) crystal has been grown using the lowtemperature modified vertical Bridgman method with slight modification in the growth setup. The design of a reformed vertical Bridgman method attached with a gear mechanism was used successfully for the growth of good optical quality TSB crystal. The grown single crystal possesses higher transparency, which proves the crystal’s suitability for scintillator and optical applications. Several growth conditions were scientifically optimized to attain improved transmittance. The thermogravimetric analysis confirms that the material is steady up to 125 °C without any phase change. The ordinary (no) and also extraordinary refractive index (ne) was evaluated by utilizing the prism coupling technique at various wavelengths in the range from 407 to 1551 nm. The neutron and gamma-ray discrimination capabilities were measured by pulse shape discrimination (PSD method) through using standard 137Cs (gamma rays) and Am–Be (neutron) radioactive sources with excellent performance. Hirshfeld surface analysis was carried out to explore the various intermolecular interactions in the TSB crystal. The maximum interaction is H…H (51.4%), which is confirmed by the abundance of hydrogen on the molecule. Results are discussed in relation to optical, structural, and scintillation properties of the grown TSB crystal. Due to its PSD ability, this crystal scintillator could be used for numerous utilizations in the division of radiation detection.