Poly- and single-crystalline BaTi2O5 co-substituted with SrO and ZrO2, Ba0.99Sr0.01(Ti1-xZrx)2O5 (BT2SZ) were prepared by arc-melting and floating-zone (FZ) melting, respectively. The specimens showed a significant (020) orientation. The highest permittivity of poly-crystalline BT2SZ was 3880 at x = 0.005 and that of single-crystal was 27000 at x = 0.005. The Curie temperature (Tc) of poly-crystals decreased from 750 to 640 K with increasing x from 0 to 0.026 and that of single-crystals decreased from 750 to 710 K with increasing x from 0 to 0.008. The highest remnant polarization of single crystalline BT2SZ was 7.8×10-2 Cm-2 at x = 0.008, higher than that of the poly-crystal.