Acrylamide (AA) is a carcinogenic, neurotoxin, and pregnancy‐harmful agent produced in food thermal processing. A specified excellent analytical technique performance is desired for detecting low AA concentration for human protection from its adverse impacts. A photoluminescent sensor APTES capped zinc oxide quantum dots (APTES/ZnO QDs) has been synthesized for AA quantification. Different capping agent's effects, for instance, triethanolamine (TEA), oleic acid (OA), tetraethyl orthosilicate (TEOS), polyvinyl pyrrolidone (PVP), 3‐aminopropyl triethoxysilane (APTES), and ethyl acetate (EA) on ZnO QDs are examined. The photoluminescence (PL) response of pristine ZnO QDs and APTES/ZnO QDs probe toward AA concentrations is investigated. This developed sensor exhibits selectivity as well as sensitivity for detecting AA ranging from 0.01 to 8.0 mM with a strong correlation coefficient (R2) of 0.9998 and a limit of detection (LOD) of 0.0019 mM, which is lesser than the WHO and European Union's guideline value. The possible photoluminescence enhancement mechanism of the APTES/ZnO QDs probe for AA detection is studied. Additionally, the reliability and performance of this facile, rapid, and precise analytical technique for quantifying AA in potato chip samples is confirmed and revealed satisfactory recoveries from 99.30 to 101.69% with relative standard deviations (RSD) from 1.4 to 1.6%.