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• we take advantage of the advantages of magnetron sputtering and pulsed laser sputtering to build a magnetron pulsed laser co-sputtering system. • By studying the VSN structure, we propose a new inverted pyramid VSN structure. • The reverse-pyramidal VSN exhibits the highest dielectric constant (428.08) and dielectric loss (0.0212) while maintaining a high tunability (78.69 %). • The inverted pyramid VSN structure improves device tuning performance and increases device lifetime. Microwaves are often used in communication engineering, including in microwave relays as well as multichannel, mobile, and satellite communications. To meet the demand for a "small, light, thin, and precise" modern electronic machine, developing highly tunable microwave materials to manufacture miniaturized microwave devices has become a top priority. Ferroelectric materials are excellent microwave materials, showing outstanding dielectric properties and tunability. Introducing low dielectric loss oxides in the construction of vertical self-assembly nanocomposites (VSNs) effectively improves their tunability and reduces dielectric loss. However, the optimal doping content of simple VSN films limits further improvement of tunability. Herein, we propose a strategy-gradient VSN to achieve combined improvement in tunability and dielectric constant by designing a sputtering and pulsed laser co-deposition. The resulting VSN composite film has a dielectric constant of 428.08, a dielectric loss of 0.0212, and a tunability of 78.69 %. Our results contribute to the development of filters and have broad application prospects in the microwave industry. we propose a strategy-gradient vertical self-assembly structure (figure c) to achieve a joint improvement in the tunability and dielectric constant (figure d) by designing a sputtering and pulsed laser codeposition (figure a). [Display omitted] [ABSTRACT FROM AUTHOR]