Pyrolysis experiments were conducted with three residua at 400 C (752 F) at various residence times. The wt% coke and gaseous products were measured for the product oils. The Western Research Institute (WRI) Coking Indexes were determined for the product oils. Measurements were made using techniques that might correlate with the Coking Indexes. These included spin-echo proton nuclear magnetic resonance spectroscopy, heat capacity measurements at 280 C (536 F), and ultrasonic attenuation. The two immiscible liquid phases that form once coke formation begins were isolated and characterized for a Boscan residuum pyrolyzed at 400 C (752 F) for 55 minutes. These materials were analyzed for elemental composition (CHNS), porphyrins, and metals (Ni,V) content.