sql insertar en la tabla con valores de casos seleccionados

Necesitas comas después de end terminando la declaración del caso. Y, el "as" va después del case declaración, no dentro de ella:

Insert into TblStuff(FullName, Address, City, Zip)
    Select (Case When Middle is Null Then Fname + LName
                 Else Fname +' ' + Middle + ' '+ Lname
            End)  as FullName,
           (Case When Address2 is Null Then Address1
                 else Address1 +', ' + Address2
            End)  as  Address,
           City as City,
           Zip as Zip
    from tblImport