MESSENGER Neutron Spectrometer (NS) observations of cosmic-ray-generated thermal neutrons provide the first direct measurements of Mercury’s surface elemental composition. Specifically, we show that Mercury’s surface is enriched in neutron-absorbing elements and has a measured macroscopic neutron-absorption cross section of 45–81×10−4 cm2/g, a range similar to the neutron absorption of lunar basalts from Mare Crisium. The expected neutron-absorbing elements are Fe and Ti, with possible trace amounts of Gd and Sm. Fe and Ti, in particular, are important for understanding Mercury’s formation and how its surface may have changed over time through magmatic processes. With neutron Doppler filtering – a neutron energy separation technique based on spacecraft velocity – we demonstrate that Mercury’s surface composition cannot be matched by prior models, which have characteristically low abundances of Fe, Ti, Gd, and Sm. While neutron spectroscopy alone cannot separate the relative contributions of individual neutron-absorbing elements, these results provide strong new constraints on the nature of Mercury’s surface materials. For example, if all the measured neutron absorption were due to the presence of an Fe–Ti oxide and that oxide were ilmenite, then Mercury’s surface would have an ilmenite content of 7–18wt.%. This result is in general agreement with the inference from color imaging and visible-near-infrared spectroscopy that Mercury’s overall low reflectance is consistent with a surface composition that is enriched in Fe–Ti oxides. The incorporation of substantial Fe and Ti in oxides would imply that the oxygen fugacity of basalts on Mercury is at the upper range of oxygen fugacities inferred for basalts on the Moon.