Taking the application merits and difficulty into consideration, a synergistical synchronous doping strategy was firstly proposed for configuring a structure stable high-performance lithium aluminum layered double hydroxide chloride type lithium adsorbents by a simple one-pot precipitation method to resist the performance attenuation of aluminum-based adsorbents during sorption. As-proposed designing strategy not only grants the LDHs-type adsorbents high adsorption capacity up to 10.4 mg/g in 400 ppm LiCl solution, but also ensures the adsorbents excellent Li+/Na+, Li+/Mg2+, Li+/K+ separation coefficients up to 236.7, 187.2 and 282.6, respectively. The initial and retained adsorption capacities after 70 desorption/adsorption cycles of as-prepared adsorbents after granulation are 12.08 and 5.09 mg/g, respectively in real sulfate-type West Taijinar Salt Lake brines with 400 ppm Li+, which is mainly attributed to the largely accelerated structure self-curability at sorption. Generally, this study can actually achieve efficient, selective and stable collection of Li+ from low-grade brines with high Mg2+/Li+ ratio.