Results of a comparative study on piezo-active 2–1–2 composites with two ferroelectric components are discussed. The composite structure combines elements of the 2–2 (laminar) and 1–3 (fibrous) connectivity patterns. The first component in each composite is domain-engineered [0 1 1]-poled single crystal with the macroscopic mm2 symmetry and high piezoelectric activity. The second component is poled ferroelectric ceramic that is represented by parallel rods in the shape of an elliptic cylinder with a large ratio of semi-axes of its base. The first orientation effect is appreciable due to rotations of the main crystallographic axes X and Y around Z || OX3 by an angle α in each crystal layer. Rotations of the ceramic rod bases by an angle γ in a polymer medium lead to the second orientation effect in the 2–1–2 composite. The two orientation effects contribute to a large anisotropy of electromechanical coupling factors k3j*, energy-harvesting figures of merit (Q3j*)2 and modified figures of merit F
3j*σ for a stress-driven harvester. The large level of (Q32*)2, (Q33*)2, F32*σ, and F33*σ (the parameters of the order of 10-11 - 10-10 Pa-1) indicates that the studied composites are suitable for piezoelectric sensors, transducers and energy-harvesting systems. New m – α diagrams put forward in the present study show regions wherein the large anisotropy of effective parameters (| k33*/ k3f*| ≥ 5, (Q33* / Q3f*)2 ≥10 and F33*σ / F3f*σ ≥ 10, f = 1 and 2) is achieved when changing the volume fraction m of single crystal and the rotation angle α. As a result, the leading role of the first orientation effect is emphasised.