The effects of particle content, size and shape on the thermal conductivity (k) and adhesion properties of thermally conductive, pressure-sensitive adhesives (PSAs) were investigated. The matrix resins were thermally crosslinkable, 2-ethylhexyl acrylic polyol and ultraviolet (UV)-curable, random copolymer consisting of acrylic oligomer and various acrylates. We found that k increased with increasing diameter and particle aspect ratio, and was further enhanced due to the reduction of the interfacial thermal barrier when the coupling agent, which increases the adhesion between particles and the matrix resin, was used. On the other hand, adhesion properties such as peel strength and tack of the thermally crosslinkable resin decreased sharply with increasing particle content. However, for UV curable resin, increased particle addition inhibited the decrease in adhesion properties.