Ok, the two files you show are not strictly "load regulation" but rather "load step transient response". They are two separate specifications. Load regulation concerns change in DC output voltage relative to dc output current. You can see a graph of that performance in the datasheet and the tolerance is very tight. It is an intrinsic property of the controller. The transient response is the change in output voltage relative to a fast acting rise or fall in load currents. While a fast acting loop will improve performance, It is generally a property of the output filter components. It is possible to improve performance by increasing the output capacitance and decreasing the output inductor value. Also you need to be sure about the load current slew rates. Fast slew rates will degrade performance. It is important to design for the actual slew rate conditions of your application. If you do in fact have fast slew rate requirements, then additional output capacitance may be required. We do have ICs that feature improved transient response. You may want to consider a device with DCAP2 control such as TPS54227 or a device with "Turbo-Trans" (I do not know a part number from memory).
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