A liquid thermal interface (LTI) including a mixture of a linearly structured polymer doped with crosslinked networks and related method are presented. The LTI exhibits reduced liquid polymer macromolecule mobility, and thus increased surface tension. An embodiment of the method includes mixing a crosslinker with a linearly structured polymer to form a mixture, wherein the crosslinker includes a base agent including a vinyl-terminated or branched polydimethylsiloxane, and a curing agent including a hydrogen-terminated polydimethylsiloxane; and curing the mixture. The crosslinker functions as cages to block linear or branched linear macromolecules and prevents them from sliding into each other, thus increasing surface tension of the resulting LTI.