Saturn's moon Titan offers great motivation for the detailed study of organic chemistry in unconventional thermodynamic conditions. Nonpolar hydrocarbons such as ethane and methane exist on Titan in plentitude, alongside one of the most prebiotically relevant and polar small molecules in existence, HCN. We here provide evidence for the intermixing of these exceptionally polar opposites at cryogenic temperatures, forming structures that defy conventional chemical expectations. Addition of hydrocarbons to HCN crystals under Titan-relevant temperatures results in small but distinct shifts in the vibrational frequencies associated with HCN. These shifts agree well with quantum mechanical calculations of co-crystal phases, which are predicted to be lower in energy compared to the pure compounds, provided some mixing and conformational disorder is permitted.