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The interface-induced second-harmonic generation from ferroelectric hafnium–zirconium oxide (Hf0.5Zr0.5O2) epitaxial thin films, buffered with a La0.67Sr0.33MnO3 bottom electrode, is analyzed as a function of input and output polarization angles and the azimuthal angle of the sample for several film thicknesses. It is shown that the signal is generated mainly from the buffer side of the interface, rather than from the ferroelectric side. However, the ferroelectric film affects significantly the nonlinear optical properties of the underlying ferromagnetic buffer electrode. Several mechanisms accounting for these observations are discussed, from oxygen migration, to an electrostatic effect, including a possible modulation of the La0.67Sr0.33MnO3 magnetization by the upper ferroelectric film. ; The authors would like to acknowledge funding from the Italian Government, PRIN-TWEET (grant code 2017YCTB59), and from the Spanish Ministry of Science and Innovation, through the Severo Ochoa FUNFUTURE (CEX2019-000917-SMCIN, AEI/10.13039/501100011033), PID2020-112548RB-I00 (MCIN/AEI/10.13039/501100011033), and PID2019-107727RB-I00 (MCIN/AEI/10.13039/501100011033) projects. All authors would like to thank Silvia Picozzi (CNR-SPIN) and Christian Rinaldi (Politecnico Milano) for the useful discussions. ; info:eu-repo/grantAgreement/AGENCIA FINANCIADORA/PROGRAMA DE FINANCIACIÓN/REFERENCIA DEL PROYECTO ; Peer reviewed