This Article explores the idea of using nonmetallic contacts for molecular electronics. Metal-free, all-carbon molecular electronic junctions were fabricated by orienting a layer of organic molecules between two carbon conductors with high yield (> 90%) and good reproducibility (rsd of current density at 0.5 V < 30%). These all-carbon devices exhibit current density-voltage (J-V) behavior similar to those with metallic Cu top contacts. However, the all-carbon devices display enhanced stability to bias extremes and greatly improved thermal stability. Completed carbon/nitroazobenzene (NAB)/carbon junctions can sustain temperatures up to 300 degrees C in vacuum for 30 min and can be scanned at +/- 1 V for at least 1.2 x 10(9) cycles in air at 100 degrees C without a significant change in J-V characteristics. Furthermore, these all-carbon devices can withstand much higher voltages and current densities than can Cu-containing junctions, which fail upon oxidation and/or electromigration of the copper. The advantages of carbon contacts stem mainly from the strong covalent bonding in the disordered carbon materials, which resists electromigration or penetration into the molecular layer, and provides enhanced stability. These results highlight the significance of nonmetallic contacts for molecular electronics and the potential for integration of all-carbon molecular junctions with conventional microelectronics.