In this paper, we consider two types of singular fractional Sturm-Liouville operators. One comprises the composition of left-sided Caputo and left-sided Riemann-Liouville derivatives of order alpha in(0,1). The other one is the composition of left-sided Riemann-Liouville and right-sided Caputo derivatives. The reality of the corresponding eigenvalues and the orthogonality of the eigenfunctions are proved. Furthermore, we formulate the fractional Laguerre Strum-Liouville problems and derive the explicit eigenfunctions as the non-polynomial functions related to Laguerre polynomials. Finally, we introduce the generalized Laguerre transform and employ it to solve the unbounded space-fractional diffusion equations.