Exfoliated MoS2 has been investigated as a dispersed catalyst for Cold Lake bitumen upgrading. The results are compared with MoS2 prepared in situ by the decomposition of molybdenum naphthenate. Although liquid yield and coke suppression were similar among the catalysts, better hydrogenation activity, especially hydrodenitrogenation, and asphaltene and microcarbon residue (MCR) removal, were obtained with the exfoliated MoS2. The improved hydrogenation is suggested to be a consequence of increased rim-edge sites associated with the exfoliated MoS2. The potential for recycle of the exfoliated MoS2 is also reported.