Herein, three sample detectors are meticulously crafted using cerium‐activated X1–Y2SiO5 (YSO:Ce3+) powder prepared via the monomer and polymer‐assisted sol–gel method. The influence of ethylene glycol (EG) monomer, polyethylene glycol polymer, and polyvinyl alcohol polymer as fuels and nucleating agents on the scintillation properties of Ce3+ (xCe = 0.01)‐doped Y2SiO5 is investigated. The sample detectors are coupled with the XP2020Q photomultiplier tube, and an advanced nuclear instrumentation system is meticulously set up for accurate measurement and characterization of scintillation properties. Scintillation decay time is precisely measured using the delayed coincidence technique under γ‐rays at 662 keV emitted from a 137Cs radioactive source. The findings underscore the significant impact of complexing agents on enhancing the scintillation performance of YSO:Ce3+ nanoscintillators. Notably, the EG‐prepared sample detector exhibits the best performance, with an estimated scintillation light yield of 22 452 ± 2600 ph MeV−1 and a coincidence timing resolution of 480 ps. These results contribute to understanding the synthesis and optimization of YSO:Ce3+ nanoscintillators for various applications, emphasizing the crucial role of the chemical environment in controlling and optimizing scintillation properties.