Powering LEDs when using Vin w/battery (Arduino Nano)

The Nano will probably run on less than 5V, and the LEDs should still light, but a little dimmer than expected.

What I suspect is that the button batteries can't provide the current required.

I suggest you try 3xAA or 3xAAA, connected directly to the 5V pin, bypassing the Nano's regulator.