Olefins are problematic components of petroleum products responsible for gum formation, polymers, and solid deposition in oil facilities. This work presents a methodology developed for monolefin analysis of whole oils, diluted bitumen, and partially upgraded heavy oils. A proton nuclear magnetic resonance ( 1 H-NMR) technique calibrated with naphtha fractions of known monolefin contents is proposed. Internal standard addition (IS, dioxane) makes the method independent of the sample C/H atomic ratios (i.e., paraffin/aromatic hydrocarbon ratios). The developed method was applied for monolefin determination of partially upgraded whole bitumen processed under mild catalytic steam cracking (CSC) conditions and is also identified as aquaprocessing (AQP). Large viscosity reductions for AQP-upgraded products (up to 99%) were determined with associated monolefin contents <1.2 wt %.