Pressure sensitive adhesives (PSAs) are polymeric materials with versatile applications in industrial and consumer products such as protective films, product labels, masking tape, and sticky notes, to name a few applications. World demand for emulsion–based products is on the rise due to worldwide legislation on solvent emissions. In order to completely replace emulsion-based PSAs with their solvent-based counterpart, the property modification of emulsion-based PSAs is required. The use of nanomaterials to modify polymer properties is well established. The aim of this thesis was to use cellulose nanocrystals (CNCs) as property modifiers for emulsion-based PSAs. CNCs are recognized as a highly efficient reinforcement nanofiller. Owing to their environmentally friendly characteristics, low density, high aspect ratio, non-toxicity, and abundant availability, the application of CNCs in composite materials is gaining increasing attention. In this thesis, the inclusion of CNCs in emulsion-based PSAs was carried out through in situ emulsion polymerization and blending technique. To the best of our knowledge, there is limited information about the synthesis of CNC/PSAs nanocomposites via in situ emulsion polymerization and the evaluation of their mechanical performance. The addition of CNCs to the polymerization formulation caused latex instability due to the negatively charged surfaces of the CNCs. After numerous attempts to overcome the stability issues, a stable polymerization formulation and protocol were developed. CNC/PSAs were synthesized via in situ seeded-semi batch emulsion polymerization, which is a common commercial production pathway for PSAs. The mechanical performance of the resulting PSA nanocomposite films, namely, shear strength, tack, and peel strength, was evaluated at several CNC loadings. All three PSA adhesive properties were simultaneously enhanced with increasing CNC loading. The inclusion of CNCs into the films increased their hydrophilicity. Consequently, the PSA films’ improved wettability on a stainless steel substrate imparted greater tack and peel strength. The blending of the CNCs with a base latex also led to improved adhesive properties. However, the property modification through blending was not as effective as that for the CNC/PSA films synthesized via in situ emulsion polymerization. Thus, CNCs are safe nanomaterials that have been shown to provide remarkable property enhancement of emulsion-based PSA films at low loadings (1wt%).