For polyacrylate latex pressure-sensitive adhesives (PSAs), high peel strength is of crucial significance. It is not only a key factor for ensuring the long-lasting and effective adhesive force of polyacrylate latex PSAs but also can significantly expand their application scope in many vital fields, such as packaging, electronics, and medical high-performance composite materials. High peel strength can guarantee that the products maintain stable and reliable adhesive performance under complex and variable environmental conditions. However, at present, the peel strength capacity of polyacrylate latex PSAs is conspicuously insufficient, making it difficult to fully meet the urgent market demand for high peel strength, and severely restricting their application in many cutting-edge fields. Therefore, based on previous experimental studies, and deeply inspired by the adhesion mechanism of natural marine mussels, in this study, a traditional polyacrylate latex PSA was ingeniously graft-modified with 3,4-dihydroxybenzaldehyde (DHBA) through the method of monomer-starved seeded semi-continuous emulsion polymerization, successfully synthesizing novel high-peel-strength polyacrylate latex pressure-sensitive adhesives (HPSAs) with outstanding strong adhesion properties, and the influence of DHBA content on the properties of the HPSAs was comprehensively studied. The research results indicated that the properties of the modified HPSAs were comprehensively enhanced. Regarding the water resistance of the adhesive film, the minimum water absorption rate was 4.33%. In terms of the heat resistance of the adhesive tape, it could withstand heat at 90 °C for 1 h without leaving residue upon tape peeling. Notably, the adhesive properties were significantly improved, and when the DHBA content reached 4.0%, the loop tack and 180° peel strength of HPSA4 significantly increased to 5.75 N and 825.4 gf/25 mm, respectively, which were 2.5 times and 2 times those of the unmodified PSA, respectively. Such superior adhesive performance of HPSAs, on the one hand, should be attributed to the introduction of the bonding functional monomer DHBA with a rich polyphenol structure; on the other hand, the acetal structure formed by the grafting reaction of DHBA with the PSA effectively enhanced the spatial network and crosslink density of the HPSAs. In summary, in this study, the natural biological adhesion phenomenon was ingeniously utilized to increase the peel strength of pressure-sensitive adhesives, providing a highly forward-looking and feasible direct strategy for the development of environmentally friendly polyacrylate latex pressure-sensitive adhesives.