The temperature (295-382 K) and pressure (5-50 Torr) dependences of the rate constants of the Al + OCS and Al + CS2 reactions have been studied by using time-resolved laser-induced fluorescence spectroscopy. The temperature dependence of the Al + OCS reaction is characteristics by the rate expression k(II)(OCS) = (4.2 +/- 2.1) x 10(-11) exp[5.3 +/- 1.4 kJ mol(-1)/RT] cm(3) molecule(-1) s(-1). The rate expression for the former reaction was found to be independent of total pressure up to 50 Torr. The pressure dependent rate expression for the reaction of Al + CS2 obeys k(III)(CS2) = (1.2 +/- 0.3) x 10(-28) Cm-6 molecule(-2) s(-1). Ab initio correlated calculations have been performed to determine the relative stability of the Al-CS2 and Al-OCS collision complexes as well as the relative energetics of reactants and products.