Nanocrystalline Ti-Fe-Co-B-based alloys, prepared by melt spinning and subsequent annealing, have been characterized structurally and magnetically. X-ray diffraction and thermomagnetic measurements show that the ribbons consist of tetragonal Ti3(Fe,Co)5B2, FeCo-rich bcc, and NiAl-rich L21 phases; Ti3(Fe,Co)5B2, is a new substitutional alloy series whose end members Ti3Co5B2 and Ti3Fe5B2 have never been investigated magnetically and may not even exist, respectively. Two compositions are considered, namely Ti11+xFe37.5-0.5xCo37.5−0.5xB14 (x = 0, 4) and alnico-like Ti11Fe26Co26Ni10Al11Cu2B14, the latter also containing an L21-type alloy. The volume fraction of the Ti3(Fe,Co)5B2 phase increases with x, which leads to a coercivity increase from 221 Oe for x = 0 to 452 Oe for x = 4. Since the grains are nearly equiaxed, there is little or no shape anisotropy, and the coercivity is largely due to the magnetocrystalline anisotropy of the tetragonal Ti3(Fe,Co)5B2 phase. The alloy containing Ni, Al, and Cu exhibits a magnetization of 10.6 kG and a remanence ratio of 0.59. Our results indicate that magnetocrystalline anisotropy can be introduced in alnico-like magnets, adding to shape anisotropy that may be induced by field annealing.