Various embodiments provide compositions that exhibit positive temperature coefficient of resistance (PTCR) properties for use in thermal interactions with tissue--including thermal sensing and I.sup.2R current-limiting interactions. Embodiments also provide tissue-engaging surfaces having PTCR materials that provide very fast switching times between low resistance and high, current-limiting resistance. One embodiment provides a matrix for an electrosurgical energy delivery surface comprising a PTCR material and a heat exchange material disposed within an interior of the matrix. The PTCR material has a substantially conductive state and a substantially non-conductive state. The heat exchange material has a structure configured to have an omni-directional thermal diffusivity for exchanging heat with the PTCR material to cause rapid switching of the PTCR material between the conductive state and non-conductive state. Preferably, the structure comprises a graphite foam having an open cell configuration. The matrix can be carried by tissue contacting surfaces of various electrosurgical devices.