Autothermal oxidative coupling of methane (OCM) is a highly attractive approach for methane utilization. If platinum-based catalysts are operated in short-contact-time reactors with high space velocities, high methane conversion can be achieved. Using a 1 wt.% Pt/Al2O3 catalyst as a benchmark, the present study elucidates how different dopants, namely Ni, Sn, and V2O5, affect the OCM reaction. Kinetic catalyst tests reveal that acetylene (C2H2) is the predominant C2 product, irrespective of the catalyst formulation or operation conditions. Furthermore, the use of bimetallic catalysts allows either for the maintenance or even the improvement of the C2 selectivity during OCM, which is attributed to synergistic effects that occur when expensive Pt is partially replaced by cheaper dopants. In particular, the 1 wt.% Pt/Al2O3 reference catalyst yielded a maximum C2 selectivity of 8.2%, whereas the best-performing doped sample 0.25 wt.% Pt 0.75 wt.% V2O5/Al2O3 yielded a total C2 selectivity of 11.3%.