If the symbols are used only in a few cases, the most efficient solution is to define \newcommand{\biggerplus}{{\myplusfont +}}, where \myplusfont is the declaration for choosing the substitute font.
If you really need to use directly + and =, then I suggest
\newfontfamily{\mytitlefont}{Some Font}
\newcommand{\choosetitlefont}{\mytitlefont\mytitlefonttrue}
\newif\ifmytitlefont
\let\pluschar=+
\catcode`+=\active
\protected\def+{\ifmytitlefont{\myplusfont\pluschar}\else\pluschar\fi}
\let\equalschar==
\catcode`==\active
\protected\def={\ifmytitlefont{\myplusfont\equalschar}\else\equalschar\fi}
Instead of calling \mytitlefont for typesetting the titles, you'll call \choosetitlefont.
Solutions with \XeTeXintercharclass would avoid activating the characters, but will have the conditional anyway.
$1+1=2$? – Leo Liu Aug 12 '11 at 11:10