AbstractWith the development of the “paper instead of plastic” trend, the investigation into high‐density, heavy‐weight paper has emerged as a point of interest in both academic and industrial realms. Regrettably, the paper‐strengthening agents that are commercially available fall short of meeting the strength specifications for such papers. To rectify this shortcoming, a water‐based acrylate paper‐strengthening agent (AA) was developed through radical emulsion polymerization. The most stable acrylate emulsion was obtained by amalgamating the anionic emulsifier allyloxyammonium oxymethyl sulfate nonylphenol ethoxy sulfate (DNS‐86) with the nonionic emulsifier nonylphenol polyoxyethylene ether (OP‐10) at a proportion of 1:0.6, with a dosage of 3%. Substituting the conventional strengthening agent (styrene‐butadiene latex) with the synthesized acrylate emulsion in wet‐end addition markedly improved the paper strength, registering a 54.8% increase to 29.4 MPa. The introduction of carboxylated cellulose nanofibers (C‐CNF) further bolstered the mechanical properties of the paper, achieving a tensile strength of 41.44 MPa and an elongation at a break of 3.55%. These results underscore the efficacy of acrylate as a paper‐strengthening agent and the crucial role of C‐CNF in enhancing the structural integrity of paper materials.