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In this paper, undoped BaBi2−x−yNb2ErxYbyO9 (BBN), Er3+ doped BBN, and a series of Er3+/Yb3+ co-doped BBN ferroelectric ceramic is synthesized by the solid-state method to study the structural, dielectric, ferroelectric, and energy storage behavior of the prepared ceramic. XRD spectra revealed orthorhombic geometry and Fmmm phase group of each prepared ceramic. SEM micrograph shows dense microstructures similar to square-shaped structures. Two FTIR bands at 619 and 822 cm−1 are observed, displaying the characteristic peaks of the Aurivillius phase. Four Raman bands are detected for undoped BBN, while twelve are visible in Er3+/Yb3+ doped BBN compositions. Further, this work utilizes a comparable method to correlate Nb–O stretching frequencies with their corresponding bond lengths using Herschbach's exponential function. Temperature-dependent dielectric studies show considerable dispersion below and above maximum temperature (Tm), and the dielectric constant (εʹ) decreases with an increase in frequency. The dielectric loss (ɛʺ) curves are quite diffused, and shifts in the maxima with frequency have been observed, thus validating the relaxor behavior of all the prepared BBN compositions. The slimmer PE curves were obtained under moderate electric fields ranging from 75 to 100 kV/cm. The energy storage parameters (W, Wrec, η) are improved with increasing applied electric field. The energy storage efficiency (η) obtained for undoped, Er3+ doped, and Er3+/Yb3+ co-doped BBN ceramics are 78.25%, 83.39%, and 90.87%, respectively. The energy storage parameters revealed good temperature stability from 303 to 415 K, indicating that the synthesized material might aid in developing modern electronic equipment for energy storage applications. [ABSTRACT FROM AUTHOR]