I have been able to create a standard Latex document using standard fonts, but merely deleting all the extra formatting hasn't worked here, so I assume there's something I don't know about going on?
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\documentclass[letter,12pt]{article} %letter paper and 12 size font default
%A Few Useful Packages
\usepackage[margin=0.9in]{geometry}
\usepackage{marvosym}
\usepackage{fontspec} %for loading fonts %%RESET
\usepackage{xunicode,xltxtra,url,parskip} %other packages for formatting
\RequirePackage{color,graphicx}
\usepackage[usenames,dvipsnames]{xcolor}
%\usepackage[big]{layaureo} %better formatting of the A4 page
% an alternative to Layaureo can be ** \usepackage{fullpage} **
\usepackage{supertabular} %for Grades
\usepackage{titlesec} %custom \section\
\usepackage{tabularx}
\usepackage{array}
\newfontfamily\smallcaps{Baskerville Small Caps SSi} %I had to DL a small caps version of Baskerville so it would work - this is the command to call that completely different font (but it's supposedly the correct matching 'small caps' font
%%reset above
\usepackage{enumitem}
\newcolumntype{R}{>{\raggedleft\arraybackslash}X}%
%This is for the Personal Data Section - not sure about using 'X'...
%Setup hyperref package, and colours for links
\usepackage{hyperref}
\definecolor{linkcolour}{rgb}{0,0.2,0.6}
\hypersetup{colorlinks,breaklinks,urlcolor=linkcolour, linkcolor=linkcolour}
%FONTS
\defaultfontfeatures{Mapping=tex-text} %% RESET
\setmainfont{Baskerville} %%reset
%CV Sections inspired by:
%http://stefano.italians.nl/archives/26
\titleformat{\section}{\Large\scshape\raggedright}{}{0em}{}[\titlerule]
\titlespacing{\section}{0pt}{3pt}{3pt}
%Tweak a bit the top margin
%\addtolength{\voffset}{-1.3cm}
\newenvironment{packed_enum}{ %THIS IS THE BULLET FORMAT FOR THE BULLET SECTIONS IN THE TABLE PART
\begin{itemize}[topsep={-10pt}, partopsep={0pt}, leftmargin={10pt}, labelindent={0pt}, itemindent={0pt}]
\setlength{\itemsep}{1pt}
\setlength{\parskip}{0pt}
\setlength{\parsep}{0pt}
}{\end{itemize}}\vspace{-\baselineskip}