A heat dissipation connection structure of handheld device includes an outer frame main body and a two-phase flow heat exchange unit. The outer frame main body has a hollow receiving space at the center. The outer frame main body surrounds the hollow receiving space. The two-phase flow heat exchange unit is disposed in the hollow receiving space and connected with the outer frame main body by means of an injection molding structure member, whereby the outer frame main body and the two-phase flow heat exchange unit can be quickly and securely connected with each other.