With increasing 3D ratio from 25 to 35%, a progressive emergence of higher-n HPs is observed, and over ~35%, a distinct phase emergence behavior consisting of 3Dlike phases (centered at ~700 nm), involving marginal n=1 and 2 2D HPs, is observed. Such phase emergence features are consistently observed up to ~90% 3D ratio. These observations indicate that, in this composition range, the BA-based 3D-like HP structures can be synthesized at a low annealing temperature (95 o C). We see inappreciable emission intensity for the compositions with over 90% 3D ratio, suggesting that thermodynamically favored non-perovskite δ-CsPbI3 crystallites, rather than 3D-like HPs, are formed. This also implies that sufficient amounts of spacer cation are vital for overcoming the thermodynamics in making 3D-like HP crystallites at such a low annealing temperature.