Let a(z) = i∈Z a i z i be a complex valued function defined for |z| = 1, such that i∈Z |ia i | < ∞, and let E = (e i,j ) i,j∈Z + be such thatToeplitz matrix associated with the symbol a(z), that is, t i,j = a j−i for i, j ∈ Z + . We analyze theoretical and computational properties of the exponential of A. More specifically, it is shown that exp(A) = T (exp(a)) + F where F = (f i,j ) i,j∈Z + is such that i,j∈Z + |f i,j | is finite, i.e., exp(A) is a semi-infinite quasi-Toeplitz matrix as well, and an effective algorithm for its computation is given. These results can be extended from the function exp(z) to any function f (z) satisfying mild conditions, and can be applied to finite quasi-Toeplitz matrices.