The polarization orientation effect and porosity effect on the piezoelectric properties and related parameters are studied in 2–2-type composites based on domain-engineered relaxor-ferroelectric [011]-poled single crystals. The parameters, which are of great interest, are an anisotropy of the piezoelectric coefficients d∗3jd∗3j, an anisotropy of the energy-harvesting figures of merit d∗3jg∗3jd∗3jg∗3j and the hydrostatic piezoelectric coefficient d∗hd∗h. An orientation of the main crystallographic axes in each polydomain single-crystal layer is described by angles ββ and γγ. Diagrams built for the first time show the (β,γβ,γ) regions, where a large anisotropy of d∗3jd∗3j (or d∗3jg∗3jd∗3jg∗3j) is achieved, and where inequality d∗h>d∗h> 1000 pC/N holds. A large local max d∗hd∗h = 1930 pC/N is achieved in a 2–2–0 PZN–0.065PT-based composite at the longitudinal piezoelectric coefficient d∗33d∗33 = 2290 pC/N and figure of merit d∗33g∗33d∗33g∗33 = 1.02..10−9−9 Pa−1−1. The aforementioned large parameters are to be of value in piezoelectric sensing, energy harvesting and hydroacoustics.