Acrylamide (AM) is a recognized carcinogen and neurotoxin, posing a significant threat to food safety and human health. Therefore, developing sensitive and convenient methods for AM detection in food samples is essential. This study responds to the urgent need for sensitive and selective detection of AM, a hidden hazard in food, to safeguard public health and environmental safety. We present the development of a novel two-dimensional ultrasound-synthesized PVP-Gd composite nanosheet platform for precise AM sensing. These self-assembled nanosheets, constructed from gadolinium (Gd) and poly(vinylpyrrolidone) (PVP), exhibit remarkable stability and robust blue fluorescence, with a quantum yield of 45.01% upon excitation at 380 nm. A full factorial design was employed to optimize the synthesis process, revealing significant parameter interactions. The optimized nanosheets demonstrated a strong quenching effect upon acrylamide exposure, resulting in a high-performance acrylamide sensor with an impressively low detection limit (9.4 nM) and a broad linear response range. This innovative sensor platform offers a promising approach for environmental monitoring and food safety applications, effectively addressing the risks associated with acrylamide.