The study of harmonic functions on a locally compact group G has recently been transferred to a "non-commutative" setting in two different directions: Chu and Lau replaced the algebra L ∞ (G) by the group von Neumann algebra VN(G) and the convolution action of a probability measure μ on L ∞ (G) by the canonical action of a positive definite function σ on VN(G); on the other hand, Jaworski and the first author replaced L ∞ (G) by B(L 2 (G)) to which the convolution action by μ can be extended in a natural way. We establish a link between both approaches. The action of σ on VN(G) can be extended to B(L 2 (G)). We study the corresponding spaceH σ of "σ -harmonic operators", i.e., fixed points in B(L 2 (G)) under the action of σ . We show, under mild conditions on either σ or G, thatH σ is in fact a von Neumann subalgebra of B(L 2 (G)). Our investigation ofH σ relies, in particular, on a notion of support for an arbitrary operator in B(L 2 (G)) that extends Eymard's definition for elements of VN(G). Finally, we present an approach toH σ via ideals in T