The narrow gap semiconductor alloys SnxGe1−x, and SnxSi1−x offer the possibility for engineering tunable direct energy gap Group IV semiconductor materials. For pseudomorphic SnxGe1−x, alloys grown on Ge (001) by molecular beam epitaxy, an indirect-to-direct bandgap transition with increasing Sn composition is observed, and the effects of misfit on the bandgap analyzed in terms of a deformation potential model. Key results are that pseudomorphic strain has only a very slight effect on the energy gap of SnxGe1−x, alloys grown on Ge (001) but for SnxGe1−x alloys grown on Ge (111) no indirect-to-direct gap transition is expected. In the SnxSi1−x system, ultrathin pseudomorphic epitaxially-stabilized α-SnxSi1−x alloys are grown on Si (001) substrates by conventional molecular beam epitaxy. Coherently strained oa-Sn quantum dots are formed within a defect-free Si (001) crystal by phase separation of the thin SnxSi1−x layers embedded in Si (001). Phase separation of the thin alloy film, and subsequent evolution occurs via growth and coarsening of regularly-shaped α-Sn quantum dots that appear as 4–6 nm diameter tetrakaidecahedra with facets oriented along elastically soft  directions. Attenuated total reflectance infrared absorption measurements indicate an absorption feature due to the α-Sn quantum dot array with onset at ˜0.3 eV and absorption strength of 8 × 103 cm−1, which are consistent with direct interband transitions.