Semiconductors with a suitable band gap and high carrier mobility are highly desirable in the electronics, optoelectronic and photovoltaic applications. The mechanical, electronic, optical and transport properties of the layered nitrides ATiN2 (A = Ca, Sr, and Ba) have been systematically studied by theoretical calculations. These nitrides show good ductility with moderate moduli, larger Poisson's ratio than 0.26 and Pugh's modulus ratio exceeding 1.75. CaTiN2 and SrTiN2 are direct bandgap semiconductors, while BaTiN2 is an indirect bandgap semiconductor, showing suitable band gaps (1.54–1.78 eV) and band edge positions for optoelectronic and photocatalytic water-splitting applications. More intriguingly, they possess superhigh carrier mobility with remarkable anisotropy. Particularly, the in-plane electron mobility reaches an ultrahigh order of 104 cm2V−1s−1, whereas those along the out-of-plane direction are almost zero. In addition, the hole mobilities are also very large along the in-plane direction and the anisotropic ratios are as high as about 30 for all these nitrides. Furthermore, these ATiN2 nitrides exhibit high optical absorption coefficients (∼105 cm−1) and lower exciton binding energies. Due to the suitable band gaps and band alignments, ultrahigh carrier mobility and huge anisotropy, excellent visible light absorption performance, the ATiN2 nitrides will be promising candidate semiconductors in electronics, optoelectronic, photovoltaic and photocatalytic applications.