Let X be a complete, simply connected harmonic manifold of purely exponential volume growth. This class contains all non-flat harmonic manifolds of non-positive curvature and, in particular all known examples of non-compact harmonic manifolds except for the flat spaces. Denote by h > 0 the mean curvature of horospheres in X, and set ρ = h / 2 . Fixing a basepoint o ∈ X , for ξ ∈ ∂ X , denote by B ξ the Busemann function at ξ such that B ξ (o) = 0 . Then for λ ∈ C the function e (i λ - ρ) B ξ is an eigenfunction of the Laplace–Beltrami operator with eigenvalue - (λ 2 + ρ 2) . For a function f on X, we define the Fourier transform of f by f ~ (λ , ξ) : = ∫ X f (x) e (- i λ - ρ) B ξ (x) d v o l (x) for all λ ∈ C , ξ ∈ ∂ X for which the integral converges. We prove a Fourier inversion formula f (x) = C 0 ∫ 0 ∞ ∫ ∂ X f ~ (λ , ξ) e (i λ - ρ) B ξ (x) d λ o (ξ) | c (λ) | - 2 d λ for f ∈ C c ∞ (X) , where c is a certain function on R - { 0 } , λ o is the visibility measure on ∂ X with respect to the basepoint o ∈ X and C 0 > 0 is a constant. We also prove a Plancherel theorem, and a version of the Kunze–Stein phenomenon. [ABSTRACT FROM AUTHOR]