The conventional cauliflower-like shape of magadiite imposes serious limitations on its applications in adsorption, catalysis, ion exchange, etc. To overcome this problem, a method to prepare it with plate-like structures was developed. This novel approach is based on an interface-controlled heterogeneous nucleation process. Zirconia grinding balls with diameters of 2.0 mm were dispersed in the starting solution to provide solid-liquid interfaces. Then the starting solution with a SiO2:NaOH:H2O molar ratio of 9:2:75 was subjected to hydrothermal treatment at 433 K for 96 h. The presence of the solid-liquid interface improved the crystallization yield and controlled the morphology and specific surface area of the crystals. With the zirconia balls, the yield and sizes of the plate-like magadiite were 52 wt.% and 1–3 μm, respectively. In the absence of zirconia balls, the yield was smaller (45 wt.%) and magadiite shaped like cauliflower was formed. The plate-like magadiite had a specific surface area of 66 m2 g−1 and a pore-size distribution between 4 and 5 nm, compared with a surface area of 28 m2 g−1 for the cauliflower-like magadiite. In addition, the plate-like magadiite was a more effective ion exchanger than the cauliflower-like magadiite with a cation exchange capacity of 64.5 mmol/100 g (compared to 53.8 mmol/100 g for the cauliflower-like form) and it had a faster sorption rate for calcium ions.