The image you posted is not made by tabular from the code you posted but probably a misused? tabular*. You can use tabular* as below but as you see, the effect of stretching the table is just to make it harder to read.

\documentclass{report}
\begin{document}
\chapter*{Camera Calibration Data, \\ Cont'd}
Focal Length in x = 953.58\\
Focal Length in y = 953.58\\
Principal Point = (959.5, 539.5)%no!\\
\begin{center}
\begin{tabular}{|c|c|c|}
\hline
Camera 1 & $\begin{array}{ccc} 0.99997 & -0.00769 & 0.00016 \\ -0.00500 & -0.66628 &-0.74569 \\ 0.00585 & 0.74567 & -0.66630 \end{array}$ & 0\\
\hline
Camera 2 & 0& 0\\
\hline
Camera 2 & 0 & 0\\
\hline
Camera 2 &0 & 0\\
\hline
Camera 2 & 0 & 0\\
\hline
Camera 2 & 0 & 0\\
\hline
\end{tabular}
\end{center}
\begin{center}
\begin{tabular*}{\textwidth}{@{\extracolsep{\fill}}|c|c|c|@{}}
\hline
Camera 1 & $\begin{array}{ccc} 0.99997 & -0.00769 & 0.00016 \\ -0.00500 & -0.66628 &-0.74569 \\ 0.00585 & 0.74567 & -0.66630 \end{array}$ & 0\\
\hline
Camera 2 & 0& 0\\
\hline
Camera 2 & 0 & 0\\
\hline
Camera 2 &0 & 0\\
\hline
Camera 2 & 0 & 0\\
\hline
Camera 2 & 0 & 0\\
\hline
\end{tabular*}
\end{center}
\end{document}
array, simply put the numbers directly into the tabular: http://pastebin.com/443JajUY – samcarter_is_at_topanswers.xyz Nov 24 '16 at 16:53