Abstract. Let X be a metric space with doubling measure, L a nonnegative self-adjoint operator in L 2 (X ) satisfying the Davies-Gaffney estimate, ω a concave function on (0, ∞) of strictly lower type p ω ∈ (0, 1] and ρ(t) = t −1 /ω −1 (t −1 ) for all t ∈ (0, ∞). The authors introduce the Orlicz-Hardy space H ω,L (X ) via the Lusin area function associated to the heat semigroup, and the BMO-type space BMO ρ,L (X ). The authors then establish the duality between H ω,L (X ) and BMO ρ,L (X ); as a corollary, the authors obtain the ρ-Carleson measure characterization of the space BMO ρ,L (X ). Characterizations of H ω,L (X ), including the atomic and molecular characterizations and the Lusin area function characterization associated to the Poisson semigroup, are also presented. Let X = R n and L = −∆ + V be a Schrödinger operator, where V ∈ L 1 loc (R n ) is a nonnegative potential. As applications, the authors show that the Riesz transform ∇L; moreover, if there exist q 1 , q 2 ∈ (0, ∞) such that q 1 < 1 < q 2 and [ω(t q 2 )] q 1 is a convex function on (0, ∞), then several characterizations of the Orlicz-Hardy space H ω,L (R n ), in terms of the Lusin-area functions, the nontangential maximal functions, the radial maximal functions, the atoms and the molecules, are obtained. All these results are new even when ω(t) = t p for all t ∈ (0, ∞) and p ∈ (0, 1).