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PACS 71.20. Lp, 75.25.+ z, 76.80.+ y Mössbauer spectroscopy has been used to investigate the hyperfine field distributions and the local spin configurations of Fe atoms in the magnetically ordered Ti(Fe 1-x Al x ) 2 compounds. The evolution of the spin arrangement of the Fe atoms was observed over the concentration range 0 ≤ x ≤ 0.25 at 5 K. The Al impurity suppresses the ferromagnetic exchange in the Fe(6h) layers and simultaneously provides the conditions for a transition of the Fe(2a) atoms, which are nonmagnetic in the TiFe 2 compound, to the states with nonzero magnetic moment. The magnetic behavior of the Fe(2a) atoms is the key factor governing the anti-to ferromagnetic transition in the Ti(Fe 1-x Al x ) 2 compounds. The magnetic ordering temperatures of the Ti(Fe 1-x Al x ) 2 compounds were determined. In addition, the parameters of the electric-field gradient in TiFe 2 as well as the relationship between the value of the magnetic moment of the Fe atom and the type of atomic configuration were discussed.