Ice growth has attracted great attention for its capability of fabricating hierarchically porous microstructure. However, the formation of tilted lamellar microstructure during freezing needs to be reconsidered due to the limited control of ice orientation with respect to the thermal gradient during in situ observations, which can greatly enrich our insight into architectural control of porous biomaterials. This paper provides an in situ study of the solid/liquid interface morphology evolution of directionally solidified single crystal ice with its C-axis (optical axis) perpendicular to directions of both the thermal gradient and the incident light in poly(vinyl alcohol, PVA) solutions. Multifaceted morphology and V-shaped lamellar morphology were clearly observed in situ for the first time. Quantitative characterizations on lamellar spacing, tilt angle, and tip undercooling of lamellar ice platelets provide a clearer insight into the inherent ice growth habit in polymeric aqueous systems and are suggested to exert significant impact on future design and optimization in porous biomaterials.