A high performance of novel three-component composites with 2–1–2 connectivity is reported and discussed. Layers of the composites are parallel-connected,and each layer contains the ferroelectric (FE) component. The layer of the first type (LFT) represents domain-engineered single crystal poled along either [0 0 1] or [0 1 1]. The layer of the second type is described as a system of long FE ceramic rods that have the shape of an elliptic cylinder and are aligned in a polymer medium. Piezoelectric coefficients $d_{3j}^{\ast }$ and $g_{3j}^{\ast }$ and sets of figures of merit (FOM) (energy-harvesting $d_{3j}^{\ast }{g}_{3j}^{\ast }$,modified $F_{3j}^{\ast \sigma }$ for a stress-driven harvester and modified $F_{3j}^{\ast \xi }$ for a strain-driven harvester) are analyzed to show their large values and specifics of the anisotropy when varying volume fractions of components and a rotation angle of the ceramic rod bases. For the first time,the studied parameters are compared in two directions: (i) the composite based on [0 0 1]-poled single crystal versus the composite based on [0 1 1]-poled single crystal and (ii) the lead-free composite versus the lead-containing composite (both based on [0 0 1]-poled single crystals). The advantages of the high-performance lead-free composite are discussed. The 2–1–2 composites put forward in this paper are of interest as advanced materials suitable for piezoelectric sensors,actuators and energy-harvesting systems operating at constant stress or strain.