Given a complex, separable Hilbert space $$\mathcal{H}$$ , we consider differential expressions of the type τ = −(d2/dx2) $$I_\mathcal{H}$$ + V(x), with x ∈ (x0,∞) for some x0 ∈ ℝ, or x ∈ ℝ (assuming the limit-point property of τ at ±∞). Here V denotes a bounded operator-valued potential V(·) ∈ $$\mathcal{B}(\mathcal{H})$$ such that V(·) is weakly measurable, the operator norm $$||V(\cdot)||_{\mathcal{B}(\mathcal{H})}$$ is locally integrable, and V(x) = V(x)* a.e. on x ∈ [x0,∞) or x ∈ ℝ. We focus on two major cases. First, on m-function theory for self-adjoint half-line L2-realizations H+,α in L2((x0,∞); dx; $$\mathcal{H}$$ ) (with x0 a regular endpoint for τ, associated with the self-adjoint boundary condition sin(α)u′(x0) + cos(α)u(x0) = 0, indexed by the selfadjoint operator α = α* ∈ $$\mathcal{B}(\mathcal{H})$$ ), and second, on m-function theory for self-adjoint full-line L2-realizations H of τ in L2(ℝ; dx; $$\mathcal{H}$$ ). In a nutshell, a Donoghue-type m-function $$M^{Do}_{A,\mathcal{N}{_i}}(\cdot)$$ associated with self-adjoint extensions A of a closed, symmetric operator $$\dot{A}$$ in $$\mathcal{H}$$ with deficiency spaces Nz = ker ( $$\dot{A}$$ * −zI $$\mathcal{H}$$ ) and corresponding orthogonal projections $${P_{{N_z}}}$$ onto Nz is given by $$\begin{gathered} M_{A,{\mathcal{N}_i}}^{Do}(z) = {P_{{\mathcal{N}_i}}}(zA + {I_\mathcal{H}})(A) - z{I_\mathcal{H}}{)^{ - 1}}{P_{{\mathcal{N}_i}|{\mathcal{N}_i}}} \hfill \\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\;\; = z{I_{{\mathcal{N}_i}}} + ({z^2} + 1){P_{{N_i}}}{(A - z{I_\mathcal{H}})^{ - 1}}{P_{{N_i}|{\mathcal{N}_i}}},\;\;\;z \in \mathbb{C}\backslash \mathbb{R}. \hfill \\ \end{gathered}$$ In the concrete case of half-line and full-line Schrodinger operators, the role of $$\dot{A}$$ is played by a suitably defined minimal Schrodinger operator H+,min in L2((x0,∞); dx; $$\mathcal{H}$$ ) and Hmin in L2(ℝ; dx; $$\mathcal{H}$$ ), both of which will be proven to be completely non-self-adjoint. The latter property is used to prove that if H+,α in L2((x0,∞); dx; $$\mathcal{H}$$ ), respectively, H in L2(ℝ; dx; $$\mathcal{H}$$ ), are self-adjoint extensions of H+,min, respectively, Hmin, then the corresponding operator-valued measures in the Herglotz–Nevanlinna representations of the Donoghue-type m-functions $$M^{Do}_{H+,\alpha},\mathcal{N_{+,i}}(\cdot)$$ and $$M^{Do}_{H,\mathcal{N}{_i}}(\cdot)$$ encode the entire spectral information of H+,α, respectively, H.