Co₂CrAl is predicted as a promising candidate for half-metallic ferromagnetism. Unfortunately, synthesis of the stoichiometric composition is a challenge as the samples prepared so far using various techniques suffer from formation of secondary phases and consequently anomalous physical properties. Off-stoichiometric compounds have been explored as a possible approach to avoid the secondary phase precipitation. The Co₂Cr_0.8Al_1.2, Co₂Cr_0.6Al_1.4 and Co₂Cr_0.4Al_1.6 compositions were synthesized using Floating Zone (FZ) technique as they melt incongruently. The secondary phase fraction was reduced as Cr was partially substituted by Al. FZ-grown Co₂Cr_0.4Al_1.6 was obtained as a single phase, signifying that the composition is out of the two-phase region. Furthermore, combining the data with an earlier work on annealing of spinodally decomposed samples, valuable insight into the extent of immiscibility was obtained.