We study projection-free methods for constrained Riemannian optimization. In particular, we pro- pose the Riemannian Frank-Wolfe (RFW) method. We analyze non-asymptotic convergence rates of Rfw to an optimum for (geodesically) convex problems, and to a critical point for nonconvex objectives. We also present a practical setting under which RFW can attain a linear convergence rate. As a concrete example, we specialize Rfw to the manifold of positive definite matrices and apply it to two tasks: (i) computing the matrix geometric mean (Riemannian centroid); and (ii) computing the Bures-Wasserstein barycenter. Both tasks involve geodesically convex interval constraints, for which we show that the Riemannian “linear oracle” required by RFW admits a closed form solution; this result may be of independent interest. We further specialize RFW to the special orthogonal group, and show that here too, the Riemannian “linear oracle” can be solved in closed form. Here, we describe an application to the synchronization of data matrices (Procrustes problem). We complement our theoretical results with an empirical comparison of RFW against state-of-the-art Riemannian optimization methods, and observe that RFW performs competitively on the task of computing Riemannian centroids.