Tailored design of high-performance nanofiltration membranes that can be used in a variety of applications such as water desalination, resource recovery, and sewage treatment is desirable. Herein, we describe the use of layered double hydroxides (LDH) intermediate layer to control the interfacial polymerization between trimesoyl chloride (TMC) and piperazine (PIP) for the preparation of polyamide (PA) membrane. The dense surface of LDH layer and its unique mass transfer behavior influence the diffusion of PIP, and the supporting role of the LDH layer allows the formation of ultrathin PA membranes. By only changing the concentration of PIP, a series of membranes with controllable thickness from 10 to 50 nm and tunable crosslinking-degree can be prepared. The membrane prepared with a higher concentration of PIP shows excellent performance for divalent salt retention with water permeance of 28 Lm⁻² h⁻¹ bar⁻¹, high rejection of 95.1 % for MgCl₂ and 97.1 % for Na₂SO₄. While the membrane obtained with a lower concentration of PIP can sieve dye molecules of different sizes with a flux of up to 70 Lm⁻² h⁻¹ bar⁻¹. This work demonstrates a novel strategy for the controllable preparation of high-performance nanofiltration membranes and provides new insights into how the intermediate layer affects the IP reaction and the final separation performance.