Abstract Problem of time-optimal control of linear systems with fractional Caputo derivatives is examined using technique of attainability sets and their support functions. A method to construct a control function that brings trajectory of the system to a strictly convex terminal set in the shortest time is elaborated. The proposed method uses technique of set-valued maps and represents a fractional version of Pontryagin’s maximum principle. A special emphasis is placed upon the problem of computing of the matrix Mittag-Leffler function, which plays a key role in the proposed methods. A technique for computing matrix Mittag-Leffler function using Jordan canonical form is discussed, which is implemented in the form of a MATLAB routine. Theoretical results are supported by examples, in which the optimal control functions, in particular of the “bang-bang” type, are obtained.