Lead-free multiferroic composites with enhanced magnetoelectric properties and sensitivity have potential for various multifunctional devices. The magnetoelectric behaviour of CoFe2O4-(Ba0.85Ca0.15) (Zr0.1Ti0.9)O3, (CFO-BCZT) and substituted CFO-BCZT laminate composites prepared by epoxy bonding are investigated in this study. Magnetostrictive CoFe2O4 (CFO) substituted with Ti (CTFO) resulted in a very high piezo-magnetic coefficient (q) of ∼290 × 10−9 Oe−1. Lead free piezoelectric (Ba0.85Ca0.15) (Zr0.1Ti0.9)O3 [BCZT] substituted with Ce4+ (BCZCT) showed improved piezoelectric coefficients of d33 ∼ 675 pC/N and g33 ∼13 mV m/N. Two new trilayer multiferroic laminates were developed with a (2-2) composite connectivity by combining the pure and substituted ferroic phases. Magnetostrictive, ferroelectric, piezoelectric and magnetoelectric properties of CFO-BCZT and CTFO-BCZCT laminate composites were measured and compared in here. CTFO-BCZCT composite exhibited a large magnetoelectric response with a high ME coefficient (αME) of ∼950 mV/cm.Oe and also showed an improved magnetoelectric sensitivity at lower magnetic fields, making it a potential lead-free material for magnetoelectric sensing applications. © 2018 Elsevier B.V.