Hydrogen has been considered as a potential candidate for the replacement of fossil fuels in future due to its renewability, abundance, ease in production, environmental friendliness and high energy efficiency. In this regard, chemical storage of hydrogen in solid state of metal hydrides is the safest method for stationary and portable applications since these can be functioned at lower pressure and ambient temperature. Among the desirable metal hydrides, the intermetallic compound TiFe of cubic CsCl-type structure is well known for absorbing hydrogen reversibly up to 1.9 wt.% to form β-FeTiH and γ-FeTiH2 phases. In this paper, we have discussed the historic background outlining the recent developments on the microstructural modifications, activation kinetics and processing routes of TiFe intermetallic alloys toward the improvement of hydrogenation properties. An in-depth microstructural analysis of TiFe alloys has been presented in terms of crystallography, hydride phase formation and hydrogenation mechanisms. The rate-controlling steps for the mechanisms of (de)hydrogenation processes of TiFe intermetallics have been explained in details. It was found that the rate-controlling steps of the hydriding reaction were dependent on the fraction of β-hydride phase. Intensive research activities were carried out to improve the first hydrogenation kinetics that can be categorized into two groups: alloying and mechanical activation. The mechanisms for improved hydrogenation kinetics in both cases have been explained. Lastly, various fabrication processes to produce TiFe alloys have been presented and correlated with cost-effectiveness and hydrogen-storage capability. Therefore, the focus of this article is to present the basic knowledge and recent developments on TiFe intermetallic alloys for future hydrogen-storage applications which will be beneficial to researchers and practitioners in the field of interest.