Sub-float package assumes that it is important to vertically align the captions, and therefore typically relies on a baseline alignment of the sub-float content.
Using adjustbox's valign=t option, the image's (the sub-float content) regular baseline alignment could be altered to now be at the top. However, you may also want to insert an appropriately-sized companion for the shorter image... do that by using \vphantom{<larger image>}:

\documentclass{article}
\usepackage[export]{adjustbox}
\usepackage{subfig}
\begin{document}
\begin{figure}
\centering
\subfloat[Part 1]{%
\includegraphics[width=0.2\textwidth,valign=t]{example-image-a}%
} \quad
\subfloat[Part 2]{%
\includegraphics[width=0.2\textwidth,valign=t]{example-image-10x16}%
}
\subfloat[Part 1]{%
\includegraphics[width=0.2\textwidth,valign=t]{example-image-a}%
\vphantom{\includegraphics[width=0.2\textwidth,valign=t]{example-image-10x16}}%
} \quad
\subfloat[Part 2]{%
\includegraphics[width=0.2\textwidth,valign=t]{example-image-10x16}%
}
\caption{Stuff will be here.}
\end{figure}
\end{document}
Package keyval Error: valign undefined. ...xtwidth,valign=t]{figures/circuitth.png}}– droid192 May 29 '19 at 11:36\usepackage[export]{adjustbox}in your preamble. Did you add that? – Werner May 29 '19 at 13:58valigninside the phantom too. I forgot this, with the result that there was lots of blank space above if you top- or center-align. – mxt3 Mar 28 '23 at 12:06