Realizing a large Landé g-factor of electrons in solid-state materials has long been thought of as a rewarding task as it can trigger abundant immediate applications in spintronics and quantum computing. Here, by using metamorphic InAsSb/InSb superlattices (SLs), we demonstrate an unprecedented high value of g ≈ 104, twice larger than that in bulk InSb, and fully spin-polarized states at low magnetic fields. In addition, we show that the g-factor can be tuned on demand from 30 to 110 via varying the SL period. The key ingredients of a large g-factor include the size of the band gap and the wavefunction overlap between the spatially separated electron and hole states, where the latter has drawn little attention in prior studies. Our work not only establishes metamorphic InAsSb/InSb as a promising and competitive material platform for future quantum devices but also provides a new route toward g-factor engineering in semiconductor structures.