Styrene-based deproteinized natural rubber (SNR) latex was synthesized by in situ polymerization. Three pre-vulcanization systems [conventional-cured (CV), semi-efficient-cured (Semi-EV), and efficient-cured (EV)] were studied in terms of tensile and adhesion properties. Good tensile properties were observed for CV and EV SNR. The Semi-EV SNR showed the best adhesion properties based on the good anchorage performance in all substrate pairings (polystyrene-polystyrene, polystyrene-rubber, and rubber-rubber). The pH modification on SNR latex via KOH addition has beneficial effects of removing protein layers, resulting in more styrene grafting sites in the rubber molecules. Consequently, the tensile and adhesion properties of the SNR are improved as more styrene polymers are grafted onto the rubber matrix. Semi-EV SNR with pH 12 has superior adhesive performance; hence, it is suitable for use as a pressure-sensitive adhesive.