This invention relates to a process for preparing laminated-column molecular sieve of crosslinking clay, including such steps as the crosslinking reaction between laminated clay (smectite kind of clay with monolayer mineral structure, or the clay with regular interstratified mineral structure) and F-containing hydroxy polymer of inorganic metal (Cr, Zr, Al, Co and Fe), ageing, washing and drying. Besides macroporous structure, such crosslinking clay has stronger acidity and higher thermal stability of acidity and acidic center, so it may be used in solid acid catalytic hydrocarbon conversion reaction.